US3632470A - Reactor fuel leak detection - Google Patents

Reactor fuel leak detection Download PDF

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Publication number
US3632470A
US3632470A US729317A US3632470DA US3632470A US 3632470 A US3632470 A US 3632470A US 729317 A US729317 A US 729317A US 3632470D A US3632470D A US 3632470DA US 3632470 A US3632470 A US 3632470A
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gas
fuel
clad
mixture
indicating
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US729317A
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Bernard F Rubin
Charles L Larson
Leonard N Grossman
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General Electric Co
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General Electric Co
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21C—NUCLEAR REACTORS
    • G21C17/00—Monitoring; Testing ; Maintaining
    • G21C17/02—Devices or arrangements for monitoring coolant or moderator
    • G21C17/04—Detecting burst slugs
    • G21C17/048—Detecting burst slugs characterised by a special construction of fuel elements, e.g. by a confined "tracer"
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E30/00—Energy generation of nuclear origin
    • Y02E30/30—Nuclear fission reactors

Definitions

  • ABSTRACT A method of detecting ruptured fuel element [52] US. Cl 176/19, cladding in nuclear reactors which permit radioactive materm 176/68 to leak therefrom is disclosed. Varying proportions of two sta- [51] lnt.C1 G21c 17/04, ble isotopes of an inert indicating gas are added to the inert G216 3/ 16 filler gas in fuel elements. Each subassembly or group of fuel [50] Field of Search 176/19, 19 demems contains a ifi individual combination f the 37 gases.
  • a typical nuclear reactor includes a chain-reacting assembly or core made up of nuclear fuel material contained in fuel elements.
  • the fuel material is encased in a corrosion-resistant heat-conductive shell or cladding.
  • the reactor core made up of a plurality of these clad fuel bodies in spaced relationship, is enclosed in a container through which the reactor coolant flows. As the coolant passes between the spaced clad fuel bodies, it is heated by thermal energy released in the fuel material during the fission reaction. The heated coolant then leaves the reactor, the thermal energy is used to perform useful work and the now-cooled coolant is recycled back to the reactor.
  • the core is generally made up of a plurality of subassemblies or bundles, each of which consists of a plurality of rod-shaped fuel elements held in a spaced parallel arrangement.
  • Each clad fuel body contains fissile material, such as U U or Pu together with an inert material and/or a fertile material such as Th or U Neutron bombardment of the fertile isotopes Th and U will produce fissile U and Pu ,-respectively.
  • the life of the fuel load will be prolonged because these created fissile materials will then fission. Where more fissile material is produced by this conversion than is consumed, the reactor is referred to as a breeder.
  • the fuel material is encased in a protective cladding of a metal such as a zirconium alloy, stainless steel, aluminum, magnesium, etc.
  • a protective cladding of a metal such as a zirconium alloy, stainless steel, aluminum, magnesium, etc.
  • the exterior surface of the cladding is in contact with a flowing stream of coolant and/or moderator, which may typically be water, steam, an organic composition such as terphenyl isomers, a liquid metal such as molten sodium, etc.
  • the cladding serves two primary purposes; first, to resist any chemical reaction between the nuclear fuel and the coo lant and/or moderator, and second, to prevent the highly radioactive fission products from being released into the coolant and/or moderator.
  • Failure of the cladding may contaminate the coolant or moderator and the coolant system with intensely radioactive long-lived fission products to a degree which interferes with plant operation and maintenance.
  • External equipment such as heat exchangers or turbines, through which the coolant passes may become contaminated.
  • reactor off-gases In a liquid-cooled system, reactor off-gases must be collected and disposed of. In wateror steam-cooled systems, these off-gases are primarily oxygen and hydrogen resulting from radiolytic decomposition of water. If these off-gases become severely contaminated by radioactive fission gases leaking from clad fuel bodies, safe disposition of the off-gases becomes difficult.
  • the gross radioactivity of the reactor coolant and/or off-gases is monitored during operation. An abrupt rise in radioactivity indicates that a cladding leak has occurred somewhere in the system. The reactor is generally shut down before excessive coolant contamination occurs.
  • the gross activity monitoring system does not, of course, indicate which of the many fuel subassemblies contains the leaking clad fuel body.
  • Another object of this invention is to provide a fuelcladding leak detection system capable of simultaneously monitoring a large number of fuel subassemblies.
  • Another object of this invention is to provide a fuelcladding leak detection system of improved sensitivity and discrimination.
  • Still another object of this invention is to provide a fuelcladding leak detection system useful within a wide variety of reactor types.
  • mixtures of an inert filler gas and an indicating gas consisting of varying proportions of two stable isotopes of another inert gas are placed in the clad fuel bodies.
  • Typical clad fuel bodies comprise an elongated closed tube substantially filled with fuel material in pellet or granular form.
  • a plenum chamber is left at one end of the tube to collect fission product gases given off by the fuel during operation in the reactor.
  • Such clad fuel bodies are described in further detail, for example, in U.S. Pat. No. 3,365,37l.
  • the plenum chamber is filled with the mixture of filler and indicating gases in accordance with this invention.
  • all of the clad fuel bodies in a single bundle or subassembly may contain the same gas mixture, since it is usually sufficient to identify the subassembly containing a leaking clad fuel body so that the subassembly may be removed from the reactor core.
  • the gas mixture must contain elements and/or isotopes which are not adversely affected by irradiation during the life of the fuel in the reactor.
  • the gases should preferably have a low neutron absorption cross section and high thermal conductivity.
  • any suitable inert gas may be used as the filler gas.
  • Typical inert gases include helium, neon, argon, krypton, and mixtures thereof. Helium is preferred, since it is readily available and has high thermal conductivity, thus aiding heat transfer from the fuel in the fuel element to the cladding.
  • the filler gas may fill both the plenum space and interstices between fuel and the cladding, as in the above gas-bonded fuel elements or may fill only the plenum space, as in sodiumbonded fuel elements where the gap between fuel and the cladding is sodium filled.
  • the bonding metal may comprise any suitable composition. Sodium, potassium, and mixtures thereof are preferred because of their excellent heat transfer properties.
  • the identifying gas to be added to the filler gas should be inert and nonreactive with the fuel material, the cladding and the coolant, must be separable from the coolant and from any cover gas used over the coolant and it should have a reasonably high thermal conductivity so as not to seriously adversely affect the thermal behavior of the fuel rods.
  • Neon has been found to meet these requirements to a high degree. Neon has three naturally occurring isotopes, Ne, Ne and Ne. These isotopes are stable and naturally occurring, with about 91 percent of natural neon in the Ne isotope and about 8 percent in the Ne isotope. The separation of these isotopes is relatively simple and both Ne and Ne are available commercially at reasonable prices.
  • Mass spectrometric analysis of isotopic ratios may readily be performed to within 0.5 percent of the neon concentration, so that Ne /Ne ratios varying by 1 percent of the total neon concentration may be discerned.
  • 10] different compositions may be prepared, ranging through 100 Ne /O percent Ne to 50 percent Ne /O percent Ne to 0 percent Ne 100 percent Ne
  • the fuel rod filler gas could comprise 90 percent He and percent of a mixture of Ne mixture and Ne. Similar ratios could be established with or percent Ne /Ne mixture and 85 or 80 percent He. A 5 percent difference in He/Ne ratio from one group to another is sufficient, since the very small amount of helium generated in the fission reaction in the fuel should not change the helium quantity by more than l2 percent.
  • This system using a mixture of helium and two neon isotopes is preferred, since it is effective, the isotopes are readily available at reasonable cost, and the concentration ratio's will not be significantly distorted by fission product gases generated in the fuel.
  • inert gases and their isotopes may be used, where suitable.
  • helium occurs in the form of two stable isotopes, He and He (although very little He occurs naturally) and argon occurs in the form of three stable isotopes, Ar, Ar and Ar"
  • the off-gases from the reactor core are desirably monitored continuously with a continuous mass spectrograph.
  • a first leak is detected, and later a second leak develops, it can be detected by the change in isotope ratio. Since generally months will pass between leaks, the probability of two rods beginning to lead at the same instant is so low as to be beyond credibility.
  • the reactor cover gas may be continuously monitored to detect an increase in concentrations of noble gas fission products such as Xe leaking from a failed fuel element.
  • a scintillation detector and multichannel analyzer may be used. Periodic samples of the cover gas, taken before and after the failure indication may be analyzed by a mass spectrograph to determine the neon or other identifying gas ratio and thus locate the failure.
  • This fuel element leak detecting system may be used in any suitable type of nuclear reactor.
  • off-gases taken off at the main condenser which primarily contain radiolytically formed hydrogen and oxygen, may be analyzed by mass spectrometry to detect the above-described filler and indicating gases leaking from a fuel element.
  • an inert cover gas such as argon, blankets the reactor core. This cover gas may be analyzed for the presence of the gas mixture from a leaking fuel element.
  • a gas such as steam or carbon dioxide
  • the coolant stream may be analyzed.
  • FIG. I there is seen a containment vessel 10 enclosing a nuclear reactor 11 and a heat exchanger 12.
  • Liquid sodium is pumped by pump 13 into reactor 11 where it passes downwardly in an annular space between shroud i4 and the wall of reactor 11.
  • the sodium then passes upwardly through core 15 which is made up of a plurality of spaced clad fuel bodies where it is heated by thermal energy given off in the fuel.
  • the reactivity of core 15 is controlled by a plurality of control rods, one of which is schematically indicated at 16.
  • the level of sodium within reactor 11 is indicated by dashed line 17.
  • Above this liquid sodium surface is a cover gas space 18, typically filled with argon.
  • the heated sodium passes through line 19 to heat exchanger 12.
  • the sodium from reactor 11 gives up heat to a second sodium stream which is pumped through coil 20 in heat exchanger 12 by pump 21.
  • the cooled reactor sodium is recycled to reactor 11 by pump 13, as described above.
  • the now-heated second sodium stream passes to steam generator 22 where the sodium in coil 23 is brought into indirect heat-exchange relationship with water to produce steam.
  • the cooled sodium is recycled to heat exchanger 12 by pump 21, as described above.
  • Radioactive material leaking from fuel elements in core 15 will contaminate the sodium coolant, reactor equipment, heat exchanger 12 and associated pumps and piping.
  • the reactor and heat exchanger have been greatly simplified in the showing of FIG. 1, for clarity. In practice they are mechanically complex. From time to time it is necessary to open the reactor for refueling and/or repair. Intense radioactive contamination makes these operations very difficult. In liquid-metal cooled reactor, sampling and analyzing coolant leaving each fuel subassembly is especially difficult because of the requirement that the sodium be maintained above its melting temperature and because sodium is a hazardous material to handle.
  • a stream of the cover gas from cover gas space 18 is pumped through line 35 by pump 36 to a detector station 37.
  • a portion of the gas stream is continuously or intermittently analyzed by a mass spectrometer for the presence of the filler and indicating gases included in the fuel rods in core 15.
  • the mass spectrometer may be designed to print a continuous gas analysis in graphic form.
  • an alarm system may be included, triggered by detection of the filler and indicating gases in the cover gas stream. Since only a small fraction of the cover gas passing through detector station 37 is consumed in the analysis, the remainder is returned to cover gas space 18 through a line 38.
  • the system does not add complex sampling equipment within the already crowded reactor vessel.
  • the detection equipment is almost entirely located outside the reactor containment, where it can be repaired or modified as necessary without shutting down the reactor. Redundancy may be provided by merely providing two detection stations 37, so that monitoring may continue while one detection station is inoperative.
  • FIG. 2 shows a schematic representation of a horizontal section through a reactor core, of the sort useful in a system such being neon-22.
  • a typical fuel subassembly in segment C, number C" in table I might contain a gas mixture consisting of 90 percent helium and i percent neon, the neon portion consisting of 87 percent neon-2O and 13 percent neon-22.
  • the fuel subassemblies or buncombinations of neon-20, neon-22 at 1 percent increments, dles have a hexagonal cross section.
  • the bundles only three different ratios of helium to neon are required using may have any other suitable cross section, such as square, 5 percent increments. This is advantageous, since helium hasa rectangular, etc.
  • the subassemblies are arranged in abutting higher thermal conductivity than neon, and is, therefore, relationship to form an overall core 150 having a generally preferred for best heat transfer characteristics. cylindrical shape.
  • Core 150 has been divided into six segments, identified by below.
  • the subassemblies having the same number in letters A through F.
  • Heavy lines delineate the segments, for each l r gm h the am n n-2 n n-22 r io. clarity.
  • the segments have rotational symmetry, that is, each However, each segment as a whole has a same neon20, neonsegment is identical with segment A, if rotated about the core 22 ratio. All of the subassemblies in each segment have the center into the position occupied by segment A.
  • the fuel subm helium/ne n r io- H w r, h gment as a whole assemblies within segment A have b b ed 101 has a helium/neon ratio different from the other segments. through 138.
  • Corresponding fuel subassemblies in segments B through F have corresponding numbers, although the numbers have been omitted from FIG. 2, for clarity.
  • Several control TABLE H elements 100 are spaced at various locations within core 110. s s These control elements 100 are conventional, vertically movag Percent gg l mom; ble, neutron-absorbing members.
  • Neon-22 Neon-20 Number Neon-22 Neon-20 Number Neon-22 Neon-20 Since there are 38 fuel subassemblies in segment A, there 0 100 81 are 228 fuel subassemblies within core 150. Thus, there must 1 99 2( go be 228 different combinations of indicating isotope ratios 3 3? 5 and/or indicating/filler gas ratios to permit positive identificag 2? tion of a subassembly containing a leaking rod by analysis of 6 b 25 75 the core off-gas. Of course, other core designs may have fewer g g? I or many more fuel subassemblies.
  • the system of this invention 9 91 5 is capable of providing many hundred identifiable gas mix- R g3 Z3 Z5 tures to accommodate any anticipated core design.
  • the gas mixture consists of helium as the 18 32 37 e filler gas and a mixture of neon-2O and neon22 as the indicat- Percent Percent 1ng gas.
  • the matrix shown 1n table I has subassembly numbers Neon Neon w1th1n each segment on the vert1cal ax1s, w1th columns for Segment mixture Helium Lsegmem mixture Hmum each lettered segment within core 110. Each column shows first the weight percent helium in the mixture, the balance g 3g 2% $2 being neon and second the weight percent of the neon-20, 15 85 30 70 neon-22 mixture which is neon-20, the balance, of course, i 7
  • each segment has the same helium/neon ratio, while each segment is rotationally the same as the others as far as location of subassemblies having the same neon-20, neon-22 ratio.
  • neon/helium ratio will identify the core segment and neon-20, neon-22 ratio will identify the subassembly within that segment which is leaking.
  • each clad fuel body a mixture comprising an inert nonradioactive elemental filler gas and an inert elemental indicating gas, said indicating gas comprising a mixture of at least two stable isotopes of said element, with at least one of l) the mass ratio of said filler gas to said indicating gas and (2) the mass ratio of said at least two isotopes in each clad fuel body being different from those in the other clad fuel bodies in said core;
  • each clad fuel body a mixture comprising an inert nonradioactive elemental filler gas and an inert elemental indicating gas, said indicating gas comprising a mixture of at least two stable isotopes of said element, said gas mixture being the same in each clad fuel body in each individual subassembly and said gas mixture being different in the clad fuel bodies in different subassemblies;
  • clad fuel bodies in at least two subassemblies contain gas mixtures dif fering in the mass ratio of said at least two isotopes of said elemental indicating gas.
  • clad fuel bodies in at least two subassemblies contain gas mixtures which differ in their mass ratio of filler gas to indicating gas.
  • a clad nuclear fuel body comprising:
  • the clad nuclear fuel body of claim 12 wherein spaces between fuel and cladding are filled with a metal selected from the group consisting os sodium, potassium and mixtures thereof and said gas mixture fills a plenum space located at one end of said body.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • Plasma & Fusion (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Monitoring And Testing Of Nuclear Reactors (AREA)
  • Examining Or Testing Airtightness (AREA)
US729317A 1968-05-15 1968-05-15 Reactor fuel leak detection Expired - Lifetime US3632470A (en)

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GB (1) GB1248489A (fr)

Cited By (15)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3856620A (en) * 1971-05-20 1974-12-24 Doryokuro Kakunenryo Kaikatsu Methods of and apparatus for detecting a failed fuel assembly
US3866043A (en) * 1970-04-20 1975-02-11 Central Electr Generat Board Coated particle fuel for nuclear reactors and to the manufacture of such fuel
US3964967A (en) * 1973-10-03 1976-06-22 The United States Of America As Represented By The United States Energy Research And Development Administration Tag gas capsule with magnetic piercing device
US4080250A (en) * 1973-11-20 1978-03-21 The United States Of America As Represented By The United States Department Of Energy Method of locating a leaking fuel element in a fast breeder power reactor
FR2377625A1 (fr) * 1977-01-12 1978-08-11 Kernenergieverwert Ges Fuer Procede d'identification des composants non etanches d'un ensemble a composants multiples
DE2925755A1 (de) * 1978-06-26 1980-01-10 Doryokuro Kakunenryo Indikatorgasfreigabeelement in einem brennstab
FR2455338A1 (fr) * 1979-04-23 1980-11-21 Tokyo Shibaura Electric Co Appareil de detection et de localisation de defaillance de combustible pour reacteur nucleaire
US4495143A (en) * 1983-09-26 1985-01-22 The United States Of America As Represented By The United States Department Of Energy Gas tagging and cover gas combination for nuclear reactor
US5473643A (en) * 1994-08-19 1995-12-05 Westinghouse Idaho Nuclear Company Corrosion testing using isotopes
US5537450A (en) * 1994-01-31 1996-07-16 Radiological & Chemical Technology, Inc. On-line analysis of fuel integrity
US6345081B1 (en) * 1997-11-21 2002-02-05 Westinghouse Atom Ab Method and a device for evaluating the integrity of the nuclear fuel in a nuclear plant
US20030185333A1 (en) * 2000-09-15 2003-10-02 Sacedon Adelantado Jose Luis Procedure and device for measuring resistance to hydriding of tubes and tubular claddings
US20050013399A1 (en) * 2001-08-23 2005-01-20 Lembit Sihver Method and a device for evaluating the integrity of a control substance in a nuclear plant
US20070134722A1 (en) * 2005-12-09 2007-06-14 Sun Microsystems, Inc. Passive tagging of products
US20070131779A1 (en) * 2005-12-09 2007-06-14 Sun Microsystems, Inc. Secure passive tagging scheme

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1640997B1 (de) * 1967-12-23 1971-06-03 Licentia Gmbh Erdungs- und Kurzschliessvorrichtung fuer elektrische Schaltanlagen
FR2191216B1 (fr) * 1972-06-28 1976-01-16 Commissariat A En Atomique Fr
US4521372A (en) * 1981-08-26 1985-06-04 Nuclear Monitoring Systems & Management Corporation Apparatus and method for monitoring stored material
DE102014118623B3 (de) 2014-12-15 2016-04-28 Areva Gmbh Vorrichtung und Verfahren zur Durchführung einer Dichtheitsprüfung an Brennstabkapseln

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1184573A (fr) * 1956-05-17 1959-07-23 élément de chauffage d'un réacteur à noyau
GB891179A (en) * 1959-07-24 1962-03-14 Atomic Energy Authority Uk Improvements in or relating to fuel elements for nuclear reactors
GB938352A (en) * 1961-08-01 1963-10-02 Atomic Energy Authority Uk Improvements in or relating to leak testing of nuclear reactor fuel elements
US3178355A (en) * 1958-05-13 1965-04-13 Gen Electric Reactor leak detector using filters

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB939714A (en) * 1961-10-17 1963-10-16 Atomic Energy Authority Uk Improvements in or relating to nuclear reactors

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR1184573A (fr) * 1956-05-17 1959-07-23 élément de chauffage d'un réacteur à noyau
US3178355A (en) * 1958-05-13 1965-04-13 Gen Electric Reactor leak detector using filters
GB891179A (en) * 1959-07-24 1962-03-14 Atomic Energy Authority Uk Improvements in or relating to fuel elements for nuclear reactors
GB938352A (en) * 1961-08-01 1963-10-02 Atomic Energy Authority Uk Improvements in or relating to leak testing of nuclear reactor fuel elements

Cited By (19)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3866043A (en) * 1970-04-20 1975-02-11 Central Electr Generat Board Coated particle fuel for nuclear reactors and to the manufacture of such fuel
US3856620A (en) * 1971-05-20 1974-12-24 Doryokuro Kakunenryo Kaikatsu Methods of and apparatus for detecting a failed fuel assembly
US3964967A (en) * 1973-10-03 1976-06-22 The United States Of America As Represented By The United States Energy Research And Development Administration Tag gas capsule with magnetic piercing device
US4080250A (en) * 1973-11-20 1978-03-21 The United States Of America As Represented By The United States Department Of Energy Method of locating a leaking fuel element in a fast breeder power reactor
FR2377625A1 (fr) * 1977-01-12 1978-08-11 Kernenergieverwert Ges Fuer Procede d'identification des composants non etanches d'un ensemble a composants multiples
DE2925755A1 (de) * 1978-06-26 1980-01-10 Doryokuro Kakunenryo Indikatorgasfreigabeelement in einem brennstab
US4495141A (en) * 1978-06-26 1985-01-22 Doryokuro Kakunenryo Kaihatsu Jigyodan Tagging gas releasing element
FR2455338A1 (fr) * 1979-04-23 1980-11-21 Tokyo Shibaura Electric Co Appareil de detection et de localisation de defaillance de combustible pour reacteur nucleaire
US4495143A (en) * 1983-09-26 1985-01-22 The United States Of America As Represented By The United States Department Of Energy Gas tagging and cover gas combination for nuclear reactor
FR2555795A1 (fr) * 1983-09-26 1985-05-31 Us Energy Combinaison perfectionnee de gaz marque et de gaz de couverture dans un reacteur nucleaire
US5537450A (en) * 1994-01-31 1996-07-16 Radiological & Chemical Technology, Inc. On-line analysis of fuel integrity
US5473643A (en) * 1994-08-19 1995-12-05 Westinghouse Idaho Nuclear Company Corrosion testing using isotopes
US6345081B1 (en) * 1997-11-21 2002-02-05 Westinghouse Atom Ab Method and a device for evaluating the integrity of the nuclear fuel in a nuclear plant
US20030185333A1 (en) * 2000-09-15 2003-10-02 Sacedon Adelantado Jose Luis Procedure and device for measuring resistance to hydriding of tubes and tubular claddings
US6873672B2 (en) * 2000-09-15 2005-03-29 Consejo Superior De Investigaciones Cientificas Procedure and device for measuring resistance to hydriding of tubes and tubular claddings
US20050013399A1 (en) * 2001-08-23 2005-01-20 Lembit Sihver Method and a device for evaluating the integrity of a control substance in a nuclear plant
US20070134722A1 (en) * 2005-12-09 2007-06-14 Sun Microsystems, Inc. Passive tagging of products
US20070131779A1 (en) * 2005-12-09 2007-06-14 Sun Microsystems, Inc. Secure passive tagging scheme
US7461793B2 (en) 2005-12-09 2008-12-09 Sun Microsystems, Inc. Secure passive tagging scheme

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DE1922592C3 (de) 1980-09-11
GB1248489A (en) 1971-10-06
DE1922592A1 (de) 1970-01-02
FR2008572A1 (fr) 1970-01-23
JPS5011556B1 (fr) 1975-05-02
DE1922592B2 (de) 1980-01-10

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